Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations

Angerer, Tina B.; Velickovic, Dusan; Nicora, Carrie D.; Kyle, Jennifer E.; Graham, Daniel J.; Anderton, Christopher R.; Gamble, Lara J.

doi:10.1021/acs.analchem.9b03763

Title: Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations

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Abstract

Lipids have been considered as key players in cell signaling and disease. Information on their location and distribution within a biological system, under varying conditions, is necessary to understand the contributions of different lipid species to an altered phenotype. Imaging mass spectrometry techniques, such as time-of-flight secondary ion mass spectrometry (ToF-SIMS) and matrix-assisted laser desorption/ionization (MALDI), are capable of revealing global lipid distributions in tissues in an untargeted fashion. Yet, to confidently identify the species present in a sample, orthogonal analyses like tandem MS (MS/MS) are often required. This can be accomplished by bulk sample analysis with liquid chromatography (LC)-MS/MS, which can provide confident lipid identifications, at the expense of losing location-specific information. Here, using planarian flatworms as a model system, we demonstrate that imaging gas cluster ion beam (GCIB)-ToF-SIMS has the unique capability to simultaneously detect, identify, and image lipid species with subcellular resolution in tissue sections. The parallel detection of both, intact lipids and their respective fragments, allows for unique identification of some species without the need of performing an additional orthogonal MS/MS analysis. This was accomplished by correlating intact lipid and associated fragment SIMS images. The lipid assignments, respective fragment identities, and locations gathered from ToF-SIMS datamore »« less

Authors:

^[1]; Velickovic, Dusan ^[2];

^[2]; Kyle, Jennifer E. ^[2]; Graham, Daniel J. ^[1];

^[2];

^[1]

Univ. of Washington, Seattle, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Publication Date:: Tue Oct 29 00:00:00 EDT 2019

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)

OSTI Identifier:: 1614990

Report Number(s):: PNNL-SA-150104
Journal ID: ISSN 0003-2700

Grant/Contract Number:: AC05-76RL01830; NNCI-1542101

Resource Type:: Accepted Manuscript

Journal Name:: Analytical Chemistry

Additional Journal Information:: Journal Volume: 91; Journal Issue: 23; Journal ID: ISSN 0003-2700

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Angerer, Tina B., Velickovic, Dusan, Nicora, Carrie D., Kyle, Jennifer E., Graham, Daniel J., Anderton, Christopher R., and Gamble, Lara J. Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations.  United States: N. p., 2019. 
Web.  doi:10.1021/acs.analchem.9b03763.

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                    Angerer, Tina B., Velickovic, Dusan, Nicora, Carrie D., Kyle, Jennifer E., Graham, Daniel J., Anderton, Christopher R., & Gamble, Lara J. Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations.  United States.  https://doi.org/10.1021/acs.analchem.9b03763

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                    Angerer, Tina B., Velickovic, Dusan, Nicora, Carrie D., Kyle, Jennifer E., Graham, Daniel J., Anderton, Christopher R., and Gamble, Lara J. Tue .  
"Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations".  United States.  https://doi.org/10.1021/acs.analchem.9b03763.  https://www.osti.gov/servlets/purl/1614990.

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@article{osti_1614990,

  title        = {Exploiting the Semidestructive Nature of Gas Cluster Ion Beam Time-of-Flight Secondary Ion Mass Spectrometry Imaging for Simultaneous Localization and Confident Lipid Annotations},

  author       = {Angerer, Tina B. and Velickovic, Dusan and Nicora, Carrie D. and Kyle, Jennifer E. and Graham, Daniel J. and Anderton, Christopher R. and Gamble, Lara J.},

  abstractNote = {Lipids have been considered as key players in cell signaling and disease. Information on their location and distribution within a biological system, under varying conditions, is necessary to understand the contributions of different lipid species to an altered phenotype. Imaging mass spectrometry techniques, such as time-of-flight secondary ion mass spectrometry (ToF-SIMS) and matrix-assisted laser desorption/ionization (MALDI), are capable of revealing global lipid distributions in tissues in an untargeted fashion. Yet, to confidently identify the species present in a sample, orthogonal analyses like tandem MS (MS/MS) are often required. This can be accomplished by bulk sample analysis with liquid chromatography (LC)-MS/MS, which can provide confident lipid identifications, at the expense of losing location-specific information. Here, using planarian flatworms as a model system, we demonstrate that imaging gas cluster ion beam (GCIB)-ToF-SIMS has the unique capability to simultaneously detect, identify, and image lipid species with subcellular resolution in tissue sections. The parallel detection of both, intact lipids and their respective fragments, allows for unique identification of some species without the need of performing an additional orthogonal MS/MS analysis. This was accomplished by correlating intact lipid and associated fragment SIMS images. The lipid assignments, respective fragment identities, and locations gathered from ToF-SIMS data were confirmed via LC-MS/MS on lipid extracts and ultrahigh mass resolution MALDI-MS imaging. Together, these data show that the semidestructive nature of ToF-SIMS can be utilized advantageously to enable both confident molecular annotations and to determine the locations of species within a biological sample.},

  doi          = {10.1021/acs.analchem.9b03763},

  journal      = {Analytical Chemistry},

  number       = 23,

  volume       = 91,

  place        = {United States},

  year         = {Tue Oct 29 00:00:00 EDT 2019},

  month        = {Tue Oct 29 00:00:00 EDT 2019}

}

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